Titanium dioxide (TiO2) particles deposited on different quantitative Fe-treated carbon nanotube (CNT) composites with high photocatalytic activity of visible light were prepared by a modified sol-gel method using TNB as a titanium source. The composites were characterized by BET, XRD, SEM, TEM and EDX, which showed that the BET surface area was related to the adsorption capacity for each composite. From TEM images, surface and structural characterization of for the CNT surface had been carried out. The XRD results showed that the Fe-ACF/TiO2 composite mostly contained an anatase structure with a Fe-mediated compound. EDX results showed the presence of C, O, and Ti with Fe peaks in the Fe-CNT/TiO2 composites. The photocatalytic activity of the composites was examined by degradation of methylene blue (MB) in aqueous solution under visible light, which was found to depend on the amount of CNT. The highest photocatalytic activity among the different composites was related to the optimal content of CNT in the Fe-CNT/TiO2 composites. In particular, the photocatalytic activity of the Fe-CNT/TiO2 composites under visible light was better than that of the CNT/TiO2 composites due to the introduction of Fe particles.